1. John T Costello National Centre for Plasma Science & Technology (NCPST)/ School of Physical Sciences, Dublin City University Multiphoton (Inner-Shell) Ionization in Intense EUV FEL Fields TPI of Xe (93 eV) and Kr (46 eV) EU COST Meeting, Krakow, 27 th -28 th May 2010 www.physics.dcu.ie/~jtc www.ncpst.ie

2. Acknowledgements Orsay: M. Meyer (now at XFEL) & D. Cubaynes (E) DESY (Hamburg): K. Tiedke, S. Düsterer, W. Li, J. Feldhaus, P. Juranić (E) PTB (Berlin): A. A. Sorokin (now at DESY), M. Richter (E) Queen’s University Belfast: Hugo W. van der Hart (T) Crete: P. Lambropoulos (T) Oulu/GSI: S. Fritzsche (T) Dublin City University: V. Richardson, J. T. Costello (E) Thanks to AG Photon (R Treusch et al.) & AG Machine (M Yurkov et al.) EU COST Meeting, Krakow, 27 th -28 th May 2010

3. Outline of Talk 1.FLASH (One slide) Overview 2.Comments on ionization in intense laser fields 3.Setup for Photoelectron Spectroscopy 4.Two Photon Ionization inner-shell of Xe (ATI) 5.Resonant Two Photon inner-shell Excitation/ Auger Decay in Kr 6.Summary / Conclusions and Next Steps EU COST Meeting, Krakow, 27 th -28 th May 2010

4. FLASH: Key Performance Indicators Ackermann et al., Nature Photonics 1 336 (2007) BL3 – allows installation of user groups focusing optics Wavelength – 4.5 nm to 60 nm Pulse Energy – 10 to 50 µJ Pulse Length – ~10s fs Photons per Pulse ~10 13

5. Ultra-dilute targets Photo-processes with ultralow cross-sections Pump and probe experiments (XUV + XUV or XUV + Opt.) Single shot measurements Few-photon single and multiple ionization processes Makes inner-shell electrons key actors in non-linear processes for the first time Re-asserts primacy of the photon over field effects ! What are the USPs of XFELs in AMOP ? EU COST Meeting, Krakow, 27 th -28 th May 2010

6. Keldysh - Ionization Regimes Multiphoton IonizationTunnel Ionization Field Ionization  >>1  ~ 2  <<1 EU COST Meeting, Krakow, 27 th -28 th May 2010 where

7. Intensity/ Wavelength Photon Energy Keldysh - Ionization Regimes Multiphoton IonizationTunnel Ionization Field Ionization  >>1  ~ 2  <<1 EU COST Meeting, Krakow, 27 th -28 th May 2010

8. FLASH@DESY offers…. High intensity - 100  J/10fs/10  m ~ 10 16 W/cm 2 Drive non-linear photoionization processes…..? Interaction with matter At high (EUV) photon energy - up to 300 eV Keldysh -  where EU COST Meeting, Krakow, 27 th -28 th May 2010

9. FLASH in the EUV - Pertubative (MPI) Regime: Ti-Sapphire in the NIR Non-Pertubative (TI) Regime So these non linear photoionization processes will involve predominantly few photons and inner and/or few electron.… Keldysh - Ionization Regime Multiphoton IonizationTunnel Ionization Field Ionization  >>1  ~ 2  <<1 Consequence - ion yield scales with intensity as I n EU COST Meeting, Krakow, 27 th -28 th May 2010

10. What’s really important about NLO/S with EUV/X-ray Lasers ? EU COST Meeting, Krakow, 27 th -28 th May 2010 Importantly - EUV/X-ray FELs bring inner shell electrons into the non- linear interaction of radiation with matter for the first time….. So Autoionising states (with femtosecond lifetimes) can play a key role in the process…. This will lead to a complex dynamical interaction between X-ray excitation and decay which means that simple ‘Single Active Electron - SAE’ models will no longer suffice…… Models that can combine and capture the physical competition between pumping and rapid (mainly) non-radiative decay of small quantum systems, along with a gamut of other parasitic/competitive NL processes (e.g., ATI) in intense EUV/X-ray fields are now needed…….

11. General EUV / XFEL AMOP Refs EU COST Meeting, Krakow, 27 th -28 th May 2010 Summary of AMOP@FLASH http://hasylab.desy.de/science/user_collaborations/amopflash 1. Photoionization Experiments with the Ultrafast XUV Laser FLASH J T Costello, J Phys Conf Ser 88 Art No 012057 (2007) 2. Experiments at FLASH C. Bostedt et al., Nucl. Inst. Meth. in Res. A 601 108 (2009) 3. Non-linear processes in the interaction of atoms and molecules with intense EUV and X-ray fields from SASE free electron lasers (FELs), N. Berrah et al., Journal of Modern Optics (in Press 2010)

12. 3. Photoelectron Spectroscopy Setup High quality, Si/Mo multi- layer mirror employed – spot size at focus ~ 4μm → 10 16 Wcm -2 (IOF-Jena) Gas Monitor Detector (GMD) provides shot-to- shot measure of FEL pulse intensity 0.65m TOF e - - spectrometer - directional magnetic field to maximise collection efficiency 93 eV …back-reflecting multilayer mirror… EU COST Meeting, Krakow, 27 th -28 th May 2010

13. 4. Xe ionization in intense XUV fields Motivation - Sorokin, Bobashev, Richter et al., PTB, PRL 2007 EU COST Meeting, Krakow, 27 th -28 th May 2010

14. One Photon Ionisation at 93 eV For low intensities (<10 14 Wcm -2 ), one photon processes are dominant Salient features – 4d photoelectron line with s/o split + Auger electron spectrum Single shot…... Not shown – 5s -1 and 5p -1 lines at higher KEs EU COST Meeting, Krakow, 27 th -28 th May 2010

15. Two Photon Inner Shell Ionisation in Xe Using MBES, first evidence of two photon inner shell ionisation, in this case of 4d electron – Xe + 2hv → Xe + 4d 9 + e - ‘Retardation field’ applied to suppress low KE electrons (one photon processes)– electron detected due solely to multiphoton events Energetically – 2 × (93) eV – 118 eV = 68 eV Yield scales quadratically, n=1.95 ±.2 EU COST Meeting, Krakow, 27 th -28 th May 2010

16. Two Photon Inner Shell Ionisation in Xe 1.However, from PRL 99 (2007) 213002 one may conclude that the FEL field produces and interacts with a highly ionized target. 2.Xe + has four 4d -1 ionization thresholds at 71.6 eV, 72.9 eV, 74.9 eV, and 76.2eV - yield photolines with KE from 110 to 115eV. However, Xe + appears only weakly in the ion spectra even at very high FEL intensity. 3.4d -1 from higher charge states also possible – outside KE region of interest 4.Additionally, two photon O-shell ionisation cross section expected to be weak from Xe 4+ & Xe 5 EU COST Meeting, Krakow, 27 th -28 th May 2010

17. 1.Using R-Matrix calculations H.W. Van der Hart) – can calculate one and two photon 4d emission partial cross sections 2.Dominant process at this KE is still one photon – ejection of next 4d – 93 eV can remove next 4d as well - or maybe 4p – removal of the second 4d electron may lead to excitation over a wide range of states. 3.Accurate calculation requires a far more substantial description of the atomic structure 4.Early estimation puts two photon 4d -1 emission at 0.5-1% of total Two Photon Inner Shell Ionisation in Xe V Richardson et al. under review at PRL

18. 5. Resonant two photon Excitation of Kr 1.To date we have looked only at non- resonant processes 2. Next phase - FEL more easily tunable, so we can now explore resonant two photon processes……. EU COST Meeting, Krakow, 27 th -28 th May 2010

19. Kr - Resonant Two Photon Excitation EU COST Meeting, Krakow, 27 th -28 th May 2010 1.Kr 3d 10 4s 2 4p 6 ( 1 S 0 ) + h (46 eV)  3d 9 4s 2 4p 6 4d (J=0,2) i.e., 3d - 4d TP excitation 2.Of course there is a direct ionization path and the usual interference results - manifested in resonance profiles (Fano/Fano-Mies) 3.But here the 3d 9 4s 2 4p 6 4d (J=0,2) resonance undergoes Auger decay to Kr+ on a femtosecond timescale - similar to the FLASH pulse duration - so competition between excitation and decay (as well as ATI makes for a complex, but intriguing, problem for theory)……

20. EU COST Meeting, Krakow, 27 th -28 th May 2010 Kr - Resonant Two Photon Excitation Kr (3d 9 4d) 2 Photon Resonance Auger MBES Photoelectron spectrum - ~ 5 x 10 14 W.cm -2 ATI Auger

21. EU COST Meeting, Krakow, 27 th -28 th May 2010 Kr - Resonant Two Photon Excitation Kr (3d 9 4d) 2 Photon Resonance Auger Theoretical Spectra – Stefan Fritzsche (GSI & Oulu)

22. EU COST Meeting, Krakow, 27 th -28 th May 2010 Kr - Resonant Two Photon Excitation Kr (3d 9 4d) 2 Photon Resonance - Ion Yield Ionization rates – P. Lambropoulos, Crete

23. EU COST Meeting, Krakow, 27 th -28 th May 2010 Kr - Resonant Two Photon Excitation Kr (3d 9 4d) 2 Photon Resonance Just out…………..

24. EU COST Meeting, Krakow, 27 th -28 th May 2010 6. Next steps: X-ray coherent control ? Ne - 2p 6 ( 1 S 0 ) Ne + - 2p 5 ( 2 P 1/2,3/2 ) Ne - 1s -1 3p( 1 P 1 ) Auger Emission Resonant ATI or RATI Rabi-Flopping AIS GS

25. EU COST Meeting, Krakow, 27 th -28 th May 2010 Next steps: X-ray coherent control ?

26. First detection of a so-called ‘above threshold ionization’ (ATI) two- photon process in an inner electron shell. Strong-field Multiple Ionization in the Inner 4d Shell by EUV Radiation The strength and the nature of the 4d → εf resonance may open up, at high irradiance, additional ionization channels, namely the simultaneous multiphoton / multi-electron from the inner 4d shell, ‘inside-out ionization’ Kr - first step on the road to resonant NL processes with EUV/X-rays…. REMPI at X-rays….. Next step - Optical pumping / coherent control at X-rays @ XFEL/LCLS Refs: Xe - Richardson et al. under review at PRL, Kr - Meyer et al., PRL (May 28 - 2010) EU COST Meeting, Krakow, 27 th -28 th May 2010 Summary